GOALI: RUI: Collaborative Research: Development of Transferable Force Fields and Monte Carlo Algorithms and Application to Phase and Sorption Equilibria

摘要1159731 eggimann， Becky L. GOALI：合作研究：可转移力场和蒙特卡罗算法的发展及其在相和吸附平衡中的应用化学和生物技术行业的可持续过程以及个人护理和洗涤剂行业的新配方的发展具有巨大的商业和环境重要性。分子水平的知识对于从基于试错的方法转向这些化学过程和配方的知识驱动设计至关重要。在这种程度上，精确的分子模型和高效的模拟算法将由Siepmann， Eggimann和Koenig领导的合作团队开发，以推进分子模拟作为高保真属性预测的工具，并提供分子水平上对相和吸收平衡的见解。将讨论与生物燃料生产和洗涤剂配方相关的具体应用。智力优点：模型开发。相平衡的可转移电位（TraPPE）家族力场将扩展到多个分辨率水平。TraPPECG（粗颗粒）将包括聚合物、沥青质和水；TraPPE吗?UA（联合原子）将添加硅氧烷和氯乙烯聚合物；TraPPEEH（显式氢）将解决环境污染物和发酵抑制剂。通过对无机离子的TraPPE盐和多孔沸石框架的TraPPE零的参数化，可以扩大预测模拟的系统和过程范围。将设计一个网络界面，以增加其他研究小组对TraPPE力场的访问。算法的发展。将开发新的蒙特卡罗算法，可以改善相转移（例如，在液-液平衡和溶液相的吸附等温线中）和微非均质流体（例如，表面活性剂系统）的空间分布的采样。应用程序。使用TraPPE力场的分子模拟将作为一种工程工具来预测各种复杂系统的热物理性质，从而增加可用的实验数据库。模拟将提供丰富的微观层面的洞察如何分子结构和组成决定宏观现象。具体来说，将进行模拟以研究(i)从发酵液中溶剂萃取乙醇，（ii）水溶液中氧合物和发酵抑制剂的吸附等温线，（iii）表面活性剂在界面和对聚电解质的吸附，（iv）胶束表面活性剂中有机物的容量限制，以及(v)混合表面活性剂双层中的相共存。更广泛的影响：研究与教育的整合。由于发现的兴奋是学生学习的重要激励因素，Siepmann和Eggimann在课堂教学（从大一的物质世界研讨会到研究生水平的统计力学）中经常整合计算练习和分子模拟研究的局部结果。Siepmann教授三年级学生的动手科学课堂，并为UMN的工程和物理科学探索项目组织了全天以计算化学为中心的活动。一个活跃的本科生研究项目是利用艾格曼促进一般的科学素养和研究作为教学的教学法。人力资源开发。通过与工业化学家的广泛互动和实际表面活性剂应用的经验，这种大学行业合作伙伴关系独特地推进了研究生和博士后的教育和培训。此外，该项目将促进大学生和高中生的参与，并特别努力从传统上代表性不足的群体中招募这些学生。对科学和工程基础设施的影响。所提出的计算研究提供的微观水平的理解将对生物燃料和表面活性剂系统的改进分离过程的设计非常有益。通过开发TraPPE力场、相关的网络工具和免费分发的MCCCS（复杂化学系统蒙特卡罗）分子模拟包，提高了计算基础设施。

Abstract1159731Eggimann, Becky L. GOALI: Collaborative Research: Development of transferable force fields and Monte Carlo algorithms and application to phase and sorption equilibriaThe development of sustainable processes in the chemical and biotechnology industries and of novel formulations in the personal care and detergent industries is of tremendous commercial and environmental importance. Molecular-level knowledge is essential for moving from trial-and-error based approaches to knowledge-driven design of these chemical processes and formulations. To this extent, accurate molecular models and efficient simulation algorithms will be developed by a collaborative team led by Siepmann, Eggimann, and Koenig to advance molecular simulation as a tool for high-fidelity property prediction and for providing molecular-level insights on phase and sorption equilibria. Specific applications relevant for biofuel production and detergent formulations will be addressed.Intellectual Merit:Model Development. The TraPPE (transferable potentials for phase equilibria) family of force fields will be extended at multiple levels of resolution. TraPPECG (coarse-grain) will include polymers, asphaltenes, and water; TraPPE?UA (united-atom) will add siloxane and vinyl chloride polymers; TraPPEEH (explicit-hydrogen) will address environmental pollutants and fermentation inhibitors. The range of systems and processes amenable to predictive simulations will be enlarged through the parameterization of TraPPE salt for inorganic ions and TraPPE zeo for porous zeolite frameworks. A web interface will be designed to increase the accessibility of the TraPPE force fieldsfor other research groups. Algorithm Development. Novel Monte Carlo algorithms will be developed that can improve the sampling of phase transfers (e.g., in liquid-liquid equilibria and sorption isotherms from solution phases) and spatial distributions in microheterogeneous fluids (e.g,, surfactant systems). Applications. Molecular simulations using the TraPPE force fields will be employed as an engineering tool to predict thermophysical properties of a variety of complex systems, thereby adding to the available experimental database. The simulations will provide a wealth of microscopic-level insight into how molecular architecture and composition determine macroscopic phenomena. Specifically, simulations will be carried out to investigate (i) the solvent-based extraction of ethanol from fermentation broths, ii) the sorption isotherms of oxygenates and fermentation inhibitors from aqueous solution, (iii) the adsorption of surfactants at interfaces and to polyelectrolytes, (iv) the capacity limit of organics in micellar surfactants, and (v) the phase coexistence in mixed surfactant bilayers.Broader Impacts:Integration of Research and Education. Because the excitement of discovery is a significant motivating factor in student learning, computational exercises and topical results from molecular simulation research are routinely integrated by Siepmann and Eggimann in their classroom teaching (spanning from of a freshman seminar on the material world to graduate-level statistical mechanics). Hands-on science classroom for third graders have been taught by Siepmann and a full day of activities centered around computational chemistry is organized for UMN's Exploring Careers in Engineering and Physical Sciences Program. An active undergraduate research program is leveraged by Eggimann to promote general scientific literacy and research-as-teaching pedagogies. Development of Human Resources. This university industry partnership uniquely advances the education and training of the graduate students and postdoctoral associates by allowing for extensive interactions with industrial chemists and experience with real-world surfactant applications. Additionally, this project will foster the participation of undergraduate and high school students, with special efforts made to recruit these students from traditionally underrepresented groups. Impact on Science and Engineering Infrastructure. The microscopic-level understanding affordedby the proposed computational investigations will be highly beneficial for the design of improved separation processes for biofuels and surfactant systems. The computing infrastructure is advanced by the development of the TraPPE force fields, the associated cybertool, and the MCCCS (Monte Carlo for Complex Chemical Systems) molecular simulation package, which are freely distributed.